<p>A facile multistep sol-gel auto combustion method was utilized to prepare a series of Mn/Gd co-substituted nano-ferrites having general chemical composition, Co_1−xMn_xGd_0.10Fe_1.90O₄; where x varies as 0.00, 0.10, 0.20, and 0.30 (with varying concentration of Mn²⁺ ions. The formation of a single-phase spinel structured nanoparticles has been confirmed from X-ray diffraction (XRD) studies. The variation in lattice constant and doping % of Mn²⁺ ions correlate well with the Vegard’s rule. The vibrational and rotational bands present between the molecules in the crystal have been determined from the FTIR and Raman spectroscopy. Raman analysis inferred the presence of five active modes illustrating the vibration of O²⁻ ions at both tetrahedral and octahedral lattice sites. The results obtained from Dielectric spectroscopy reveals the Maxwell Wagner Polarization with the dielectric permittivity (ε´) values increased from 32.790 to 903.932 with the subsequent rise in doping % of Mn²⁺ ions. In the low frequency regime, the reduction in dielectric loss values from 20971.62 to 400 has been attributed upon increased addition of Mn²⁺ ions. The AC conductivity revealed the involvement of small polaron hopping in causing the electrical conduction with the successive increment from 6.29 E-08 (100&#xa0;Hz, x = 0.00) to 1.405 E-07 (100&#xa0;Hz, x = 0.30). The ferroelectric measurements yielded improved in the saturation polarization from 3.216 µC/cm² to 12.185 µC/cm² with the increase in Mn²⁺ ions substitution. The obtained results provide a wide range of possibilities for the practical use of these materials for developing high frequency devices with high polarizability.</p>